During the 2011 Tour de France, Rolland gained acclaim for his strong work in defense of Thomas Voeckler's yellow jersey. Following the 14th stage of the Tour, Lance Armstrong referred to Rolland as a "rockstar."[4] Rolland won the 19th stage at the top of Alpe d'Huez, beating Olympic gold medalist Samuel Sánchez and two-time Tour champion Alberto Contador.[5] The victory also won him the white jersey, which he successfully defended in the 20th stage. He finished the Tour 10th in the general classification.

At the 2012 Tour de France, Rolland made a late attack which led to him winning stage 11, a mountain top finish up in La Toussuire/Les Sybelles.[6] He finished the Tour in eighth place in the general classification, his best career performance, and the highest position of any Frenchman that year.